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Covalent triazine framework supported non-noble metal nanoparticles with superior activity for catalytic hydrolysis of ammonia borane: from mechanistic study to catalyst design.

ABSTRACT: Development of non-noble metal catalysts with similar activity and stability to noble metals is of significant importance in the conversion and utilization of clean energy. The catalytic hydrolysis of ammonia borane (AB) to produce 3 equiv. of H₂, as an example of where noble metal catalysts significantly outperform their non-noble peers, serves as an excellent test site for the design and optimization of non-noble metal catalysts. Our kinetic isotopic effect measurements reveal, for the first time, that the kinetic key step of the hydrolysis is the activation of H₂O. Deducibly, a transition metal with an optimal electronic structure that bonds H₂O and -OH in intermediate strengths would favor the hydrolysis of AB. By employing a covalent triazine framework (CTF), a newly developed porous material capable of donating electrons through the lone pairs on N, the electron densities of nano-sized Co and Ni supported on CTF are markedly increased, as well as their catalytic activities. Specifically, Co/CTF exhibits a total turnover frequency of 42.3 mol_H₂ mol_Co^-1 min^-1 at room temperature, which is superior to all peer non-noble metal catalysts ever reported and even comparable to some noble metal catalysts.

SUBMITTER: Li Z

PROVIDER: S-EPMC5299936 | biostudies-literature |

REPOSITORIES: biostudies-literature

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A Three-Stage Mechanistic Model for Ammonia Borane Dehydrogenation by Shvo's Catalyst.

Project description:We propose a mechanistic model for three-stage dehydrogenation of ammonia borane (AB) catalyzed by Shvo's cyclopentadienone-ligated ruthenium complex. We provide evidence for a plausible mechanism for catalyst deactivation, the transition from fast catalysis to slow catalysis, and relate those findings to the invention of a second-generation catalyst that does not suffer from the same deactivation chemistry.The primary mechanism of catalyst deactivation is borazine-mediated hydroboration of the ruthenium species that is the active oxidant in the fast catalysis case. This transition is characterized by a change in the rate law for the reaction and changes in the apparent resting state of the catalyst. Also, in this slow catalysis situation, we see an additional intermediate in the sequence of boron, nitrogen species, aminodiborane. This occurs with concurrent generation of NH(3), which itself does not strongly affect the rate of AB dehydrogenation.

| S-EPMC3546831 | biostudies-literature

Hexagonal CuCo₂O₄ Nanoplatelets, a Highly Active Catalyst for the Hydrolysis of Ammonia Borane for Hydrogen Production.

Project description:Catalytic hydrolysis of ammonia borane (AB) has been considered as an effective and safe method to generate hydrogen. Development of highly active and low-cost catalysts is one of the key tasks for this technology. In this work, hexagonal CuCo₂O₄ nanoplatelets with a thickness of approximately 55 nm were prepared. In AB hydrolysis, those nanoplatelets exhibited ultrahigh catalytic activity with turnover frequency (TOF) of 73.4 molhydrogen min-1 molcat-1. As far as we know, this is one of the highest TOF values ever reported for non-noble metal catalysts. In addition, the effects of viscosity and different alkalis on the hydrolysis were also investigated. It is revealed that high viscosity of the reaction medium will retard the hydrolysis reaction. The presence of NaOH, KOH, and Na₂CO₃ in the reaction solution is favorable for hydrolytic process. In contrast, NH₃·H₂O will slow down the hydrolysis rate of ammonia borane. This work can provide some novel insight into the design of catalysts with both high performance and low cost. Besides, some findings in the present study can also offer us some information about how to improve the hydrolysis rates by optimizing the hydrolysis condition.

| S-EPMC6473973 | biostudies-literature

Bracelet-Like Ni<sub>0.4</sub>Cu<sub>0.6</sub>O Microstructure Composed of Well-Aligned Nanoplatelets as a Superior Catalyst to the Hydrolysis of Ammonia Borane.

Project description:The development of novel catalysts with both high catalytic activity and low cost toward the hydrolysis of ammonia borane is an important subject in the field of hydrogen energy. In this communications, NixCu1-xO microstructures with different morphology have been synthesized and their catalytic activities in AB hydrolysis is studied. It's found that bracelet-like nanoplatelets were obtained at x = 0.4 and exhibit highest catalytic performance with turnover frequency of 33.43 molhydrogen min-1 mol cat - 1 , which much higher than those of most of CuNi-based catalysts in the literature. Pronounced synergistic effects between CuO and NiO in AB hydrolysis also have been observed. Due to the superior catalytic performance and cheapness, the prepared bracelet-like nanoplatelets Ni0.4Cu0.6O catalysts can be a strong catalyst candidate in AB hydrolysis.

| S-EPMC6868442 | biostudies-literature

Metal Ruthenate Perovskites as Heterogeneous Catalysts for the Hydrolysis of Ammonia Borane.

Project description:Ammonia borane (NH3-BH3) is of interest as a hydrogen storage material because of its ease of use and its ability to release three molar equivalents of H2(g) via catalytic hydrolysis. Most heterogeneous catalysts for ammonia borane hydrolysis are nanoparticles containing expensive noble metals. Here, we show that metal ruthenate perovskites function as active and durable catalysts for ammonia borane hydrolysis. As a bulk powder, CaRuO3 catalyzes the hydrolysis of ammonia borane at room temperature and is recyclable and reusable. CaRuO3 facilitates the release of H2(g) from aqueous ammonia borane solutions at comparable rates to some other heterogeneous catalyst systems while having a low noble metal content. Other ruthenium-based perovskites, including SrRuO3, Ca2LaRuO6, Sr2CoRuO6, and SrLaCoRuO6, are similarly active catalysts for room-temperature ammonia borane hydrolysis.

| S-EPMC6641281 | biostudies-literature

TiN nanotube supported Ni catalyst Ni@TiN-NTs: experimental evidence of structure-activity relations in catalytically hydrolyzing ammonia borane for hydrogen evolution.

Project description:With commercial TiO2 as the precursor, titanium nitride nanotubes (TiN-NTs) were fabricated through a hydrothermal - ammonia nitriding route, and next non-noble metal nanosized Ni particles were evenly and firmly anchored on the surface of the TiN-NTs via a PVP-mediated non-aqueous phase reduction-deposition strategy, to obtain the supported catalyst Ni@TiN-NTs. The X-ray powder diffraction (PXRD), field emission scanning and transmission electron microscopy (FE-SEM/TEM) and specific surface area measurements were used to characterize and analyze the phase composition, surface microstructure and morphological features of the product. The catalytic activity of the Ni@TiN-NTs for hydrolyzing ammonia borane to generate hydrogen (H2) under different conditions was evaluated systematically. The results reveal that the as-fabricated TiN-NTs are composed of TiN and a small amount of TiN x O y with the approximate molar atomic ratio of Ti to N at 1 : 1, existing as hollow microtubules with mean tube diameter of 130 nm and length of about 1 μm. Via in situ reduction and deposition, Ni nanoparticles can be uniformly anchored on the surface of TiN-NTs. The catalytic activities of Ni(x)@TiN-NTs with different Ni loading amounts are all higher than that of single metal Ni nanoparticles. The temperature has a positive effect on the catalytic activity of Ni(20)@TiN-NTs, and its total turnover frequency for hydrolyzing ammonia borane is 11.73 mol(H2) (mol Ni)-1 min-1, with an apparent activation energy of 52.05 kJ mol-1 at 303 K. After 5 cycles, the Ni(20)@TiN-NTs catalyst still maintains 87% of the initial catalytic activity. It could be suggested that these tactics can also be extended to the fabrication of other metal or alloy catalysts supported by TiN-NTs, with great application potential and development prospects.

| S-EPMC9057120 | biostudies-literature

A robust, air-stable, reusable ruthenium catalyst for dehydrogenation of ammonia borane.

Project description:We describe an efficient homogeneous ruthenium catalyst for the dehydrogenation of ammonia borane (AB). This catalyst liberates more than 2 equiv of H(2) and up to 4.6 system wt % H(2) from concentrated AB suspensions under air. Importantly, this catalyst is robust, delivering several cycles of dehydrogenation at high [AB] without loss of catalytic activity, even with exposure to air and water.

| S-EPMC3168700 | biostudies-literature

Ruthenium nanoparticles confined in SBA-15 as highly efficient catalyst for hydrolytic dehydrogenation of ammonia borane and hydrazine borane.

Project description:Ultrafine ruthenium nanoparticles (NPs) within the mesopores of the SBA-15 have been successfully prepared by using a "double solvents" method, in which n-hexane is used as a hydrophobic solvent and RuCl3 aqueous solution is used as a hydrophilic solvent. After the impregnation and reduction processes, the samples were characterized by XRD, TEM, EDX, XPS, N2 adsorption-desorption, and ICP techniques. The TEM images show that small sized Ru NPs with an average size of 3.0 ± 0.8 nm are uniformly dispersed in the mesopores of SBA-15. The as-synthesized Ru@SBA-15 nanocomposites (NCs) display exceptional catalytic activity for hydrogen generation by the hydrolysis of ammonia borane (NH3BH3, AB) and hydrazine borane (N2H4BH3, HB) at room temperature with the turnover frequency (TOF) value of 316 and 706 mol H2 (mol Ru min)(-1), respectively, relatively high values reported so far for the same reaction. The activation energies (Ea) for the hydrolysis of AB and HB catalyzed by Ru@SBA-15 NCs are measured to be 34.8 ± 2 and 41.3 ± 2 kJ mol(-1), respectively. Moreover, Ru@SBA-15 NCs also show satisfied durable stability for the hydrolytic dehydrogenation of AB and HB, respectively.

| S-EPMC4607937 | biostudies-literature

Ammonia-triphenyl-borane.

Project description:The asymmetric unit of the title compound, C(18)H(18)BN or (C(6)H(5))(3)B·NH(3), comprises two crystallographically independent but virtually identical mol-ecules. Mol-ecules of one type are linked with each other by N-H⋯π inter-actions, generating an infinite column aligned along the b-axis direction. The columns of different types of mol-ecules are inter-connected by C-H⋯π inter-actions, producing a three-dimensional array.

| S-EPMC3247484 | biostudies-literature

Catalytic Behavior of Iron-Containing Cubic Spinel in the Hydrolysis and Hydrothermolysis of Ammonia Borane.

Project description:The paper presents a comparative study of the activity of magnetite (Fe3O4) and copper and cobalt ferrites with the structure of a cubic spinel synthesized by combustion of glycine-nitrate precursors in the reactions of ammonia borane (NH3BH3) hydrolysis and hydrothermolysis. It was shown that the use of copper ferrite in the studied reactions of NH3BH3 dehydrogenation has the advantages of a high catalytic activity and the absence of an induction period in the H2 generation curve due to the activating action of copper on the reduction of iron. Two methods have been proposed to improve catalytic activity of Fe3O4-based systems: (1) replacement of a portion of Fe2+ cations in the spinel by active cations including Cu2+ and (2) preparation of highly dispersed multiphase oxide systems, involving oxide of copper.

| S-EPMC8468860 | biostudies-literature

A Highly Active Bidentate Magnesium Catalyst for Amine-Borane Dehydrocoupling: Kinetic and Mechanistic Studies.

Project description:A magnesium complex (1) featuring a bidentate aminopyridinato ligand is a remarkably selective catalyst for the dehydrocoupling of amine-boranes. This reaction proceeds to completion with low catalyst loadings (1 mol %) under mild conditions (60 °C), exceeding previously reported s-block systems in terms of selectivity, rate, and turnover number (TON). Mechanistic studies by in situ NMR analysis reveals the reaction to be first order in both catalyst and substrate. A reaction mechanism is proposed to account for these findings, with the high TON of the catalyst attributed to the bidentate nature of the ligand, which allows for reversible deprotonation of the substrate and regeneration of 1 as a stable resting state.

| S-EPMC6563444 | biostudies-literature

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